John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, 02138, USA.
Wyss Institute for Biologically Inspired Engineering, Harvard University, Boston, MA, 02115, USA.
Adv Mater. 2021 Apr;33(17):e2008553. doi: 10.1002/adma.202008553. Epub 2021 Mar 24.
The development of tough adhesive hydrogels has enabled unprecedented adhesion to wet and moving tissue surfaces throughout the body, but they are typically composed of nondegradable components. Here, a family of degradable tough adhesive hydrogels containing ≈90% water by incorporating covalently networked degradable crosslinkers and hydrolyzable ionically crosslinked main-chain polymers is developed. Mechanical toughness, adhesion, and degradation of these new formulations are tested in both accelerated in vitro conditions and up to 16 weeks in vivo. These degradable tough adhesives are engineered with equivalent mechanical and adhesive properties to nondegradable tough adhesives, capable of achieving stretches >20 times their initial length, fracture energies >6 kJ m , and adhesion energies >1000 J m . All degradable systems show complete degradation within 2 weeks under accelerated aging conditions in vitro and weeks to months in vivo depending on the degradable crosslinker selected. Excellent biocompatibility is observed for all groups after 1, 2, 4, 8, and 16 weeks of implantation, with minimal fibrous encapsulation and no signs of organ toxicity. On-demand removal of the adhesive is achieved with treatment of chemical agents which do not cause damage to underlying skin tissue in mice. The broad versatility of this family of adhesives provides the foundation for numerous in vivo indications.
坚韧的可降解水凝胶的发展使人们能够以前所未有的黏附力黏附于全身的湿润和运动组织表面,但这些水凝胶通常由不可降解的成分组成。在这里,我们开发了一类可降解的坚韧的水凝胶,其中含有约 90%的水,通过掺入共价交联的可降解交联剂和可水解的离子交联主链聚合物。在体外加速条件下和体内长达 16 周的时间内,对这些新配方的机械韧性、黏附力和降解性能进行了测试。这些可降解的坚韧黏附剂具有与不可降解的坚韧黏附剂相当的机械和黏附性能,能够实现超过初始长度 20 倍的拉伸、超过 6kJ/m 的断裂能和超过 1000J/m 的黏附能。所有的可降解体系在体外加速老化条件下 2 周内完全降解,在体内则根据所选的可降解交联剂在数周到数月内降解。所有组在植入后 1、2、4、8 和 16 周均表现出良好的生物相容性,仅有最小的纤维包裹,没有器官毒性的迹象。通过用化学试剂处理,可以实现对黏附剂的按需去除,而这些化学试剂不会对小鼠的皮肤组织造成损伤。这种黏附剂家族的广泛多功能性为许多体内应用提供了基础。